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Physical Review A

Transient absorption spectra of the laser-dressed hydrogen atom

Mitsuko Murakami, Shih‐I Chu

Published Oct 28, 2013• 12 citations
Publisher

Abstract

We present a theoretical study of transient absorption spectra of laser-dressed hydrogen atoms, based on numerical solutions of the time-dependent Schr\"odinger equation. The timing of absorption is controlled by the delay between an extreme ultra violet (XUV) pulse and an infrared (IR) laser field. The XUV pulse is isolated and several hundred attoseconds in duration, which acts as a pump to drive the ground-state electron to excited $p$ states. The subsequent interaction with the IR field produces dressed states, which manifest as sidebands between the 1s-$np$ absorption spectra separated by one IR-photon energy. We demonstrate that the population of dressed states is maximized when the timing of the XUV pulse coincides with the zero crossing of the IR field, and that their energies can be manipulated in a subcycle time scale by adding a chirp to the IR field. An alternative perspective to the problem is to think of the XUV pulse as a probe to detect the dynamical ac Stark shifts. Our results indicate that the accidental degeneracy of the hydrogen excited states is removed while they are dressed by the IR field, leading to large ac Stark shifts. Furthermore, we observe the Autler-Townes doublets for the $n=2$ and 3 levels using the 656 nm dressing field, but their separation does not agree with the prediction by the conventional three-level model that neglects the dynamical ac Stark shifts.

DOI
10.1103/physreva.88.043428

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We present a theoretical study of transient absorption spectra of laser-dressed hydrogen atoms, based on numerical solutions of the time-dependent Schr"odinger equation. The timing of absorption is controlled by the delay between an extreme ultra violet (XUV) pulse and an infrared (IR) laser field. The XUV pulse is isolated and several hundred attoseconds in duration, which acts as a pump to drive the ground-state electron to excited ppp states. The subsequent interaction with the IR field produces dressed states, which manifest as sidebands between the 1s-npnpnp absorption spectra separated by one IR-photon energy. We demonstrate that the population of dressed states is maximized when the timing of the XUV pulse coincides with the zero crossing of the IR field, and that their energies can be manipulated in a subcycle time scale by adding a chirp to the IR field. An alternative perspective to the problem is to think of the XUV pulse as a probe to detect the dynamical ac Stark shifts. Our results indicate that the accidental degeneracy of the hydrogen excited states is removed while they are dressed by the IR field, leading to large ac Stark shifts. Furthermore, we observe the Autler-Townes doublets for the n=2n=2n=2 and 3 levels using the 656 nm dressing field, but their separation does not agree with the prediction by the conventional three-level model that neglects the dynamical ac Stark shifts.
We present a theoretical study of transient absorption and reshaping of extreme ultraviolet (XUV) pulses by helium atoms dressed with a moderately strong infrared (IR) laser field. We formulate the atomic response using both the frequency-dependent absorption cross section and a time-frequency approach based on the time-dependent dipole induced by the light fields. The latter approach can be used in cases when an ultrafast dressing pulse induces transient effects, and/or when the atom exchanges energy with multiple frequency components of the XUV field. We first characterize the dressed atom response by calculating the frequency-dependent absorption cross section for XUV energies between 20 and 24 eV for several dressing wavelengths between 400 and 2000 nm and intensities up to 1012{}^{12}12 W/cm2{}^{2}2. We find that for dressing wavelengths near 1600 nm, there is an Autler-Townes splitting of the $1s\ensuremath{\rightarrow}2p$ transition that can potentially lead to transparency for absorption of XUV light tuned to this transition. We study the effect of this XUV transparency in a macroscopic helium gas by incorporating the time-frequency approach into a solution of the coupled Maxwell-Schr\"odinger equations. We find rich temporal reshaping dynamics when a 61-fs XUV pulse resonant with the $1s\ensuremath{\rightarrow}2p$ transition propagates through a helium gas dressed by an 11-fs, 1600-nm laser pulse.
In the present paper, we investigate the time-resolved transient absorption spectroscopy of doubly excited states of helium atoms by solving the time-dependent two-electron Schr\"odinger equation numerically based on a one-dimensional model. The helium atoms are subjected to an extreme ultraviolet (XUV) attosecond pulse and a time-delayed infrared (IR) few-cycle laser pulse. A superposition of doubly excited states populated by the XUV pulse is identified, which interferes with the direct ionization pathway leading to Fano resonance profiles in the photoabsorption spectrum. In the presence of an IR laser, however, the Fano line profiles are strongly modified: A shifting, splitting, and broadening of the original absorption lines is observed when the XUV attosecond pulse and infrared few-cycle laser pulse overlap in time, which is in good agreement with recent experimental results. At certain time delays, we observe symmetric Lorentz, inverted Fano profiles, and even negative absorption cross sections indicating that the XUV light can be amplified during the interaction with atoms. We further prove that the above pictures are general for different doubly excited states by suitably varying the frequency of the IR field to coherently couple the corresponding states.
We present a theoretical study of the transient absorption of an ultrafast, extreme ultraviolet (XUV) pulse in the presence of an infrared (IR) control pulse in a macroscopic three-level helium gas. We concentrate on cases in which the IR pulse is shorter than the XUV pulse and induces transient transparency and amplification of the XUV light via coherent control. We give a time-dependent picture of the absorption process through the time dependence of the populations and relative coherences of the three states. We show that the XUV absorption can be dynamically changed into emission via phase control of the XUV-resonant 2p2p2p state through IR-induced coupling between the 2p2p2p and the 2s2s2s states. This can lead to compression and amplification of the XUV pulse when propagating through a laser-dressed macroscopic medium. We discuss the influence of atomic decoherence times on the XUV reshaping and show that fast decoherence means that the laser dressing acts more like a passive transmission window and less like a dynamical redistribution of energy.
We calculate the transient absorption of an isolated attosecond pulse (IAP) by helium atoms subject to a delayed infrared (IR) laser pulse. With the central frequency of the broad attosecond spectrum near the ionization threshold, the absorption spectrum is strongly modulated at the sub-IR-cycle level. Given that the absorption spectrum results from a time-integrated measurement, we investigate the extent to which the delay dependence of the absorption yields information about the attosecond dynamics of the atom-field energy exchange. We find two configurations in which this is possible. The first involves multiphoton transitions between bound states that result in interference between different excitation pathways. The second involves the modification of the bound state absorption lines by the IR field, which we find can result in a subcycle time dependence only when ionization limits the duration of the strong-field interaction.
We theoretically investigate the attosecond transient absorption spectrum of helium atom in the presence of an infrared-dressed laser pulse upon scanning their relative delay, with the particular emphasis on the chirp effect of the attosecond pulse. By numerically solving the fully three-dimensional time-dependent Schrödinger equation, we identify the attoscecond chirp can induce the temporal shift of the absorption spectrogram along the delay axis. Additionally, it is found that the extent of the temporal shift is dependent on both the position of the absorption line and the infrared pulse wavelength, which is well confirmed and reproduced by a three-level model. Moreover, we demonstrate that the observed features can be quantitatively explained in terms of the indirect two-photon absorption processes through some virtual states. This effect might provide a way to measure the chirp of attosecond pulse in an all-optical way.
In the present paper, the time-resolved transient absorption spectroscopy of helium atoms is investigated based on the three-level modeling. The helium atoms are subjected to an extreme ultraviolet (XUV) attosecond pulse and a time-delayed infrared (IR) few-cycle laser field. The odd excited state are populated from the ground state by the XUV pulse due to the dipole selection rule, and probed by the time-delayed IR laser. The time-resolved transient absorption spectroscopy based on the different coupling mechanism demonstrate some different features, the photoabsorption spectrum based on three-level model with rotating wave approximation (RWA) cannot repeat the fast oscillation and the sideband structure which have been observed in the previous experimental investigation. The dressing effect of IR laser pulse on the ground state can contribute new interference structures in the photoabsorption spectrum.